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20-22, 2009

and Application to Limestone Calcination

Uwe Kssel1 Dirk Abel1 Matthias Schumacher2 Martin Weng2

1 RWTH Aachen University, Institute of Automatic Control

Steinbachstrae 54A, D-52074 Aachen

2 Aixprocess, Process and Fluid Engineering

Alfonsstrasse 44, D-52070 Aachen

Abstract

become available to close the control loop. To be applicable to an expert system, the very complex model

This paper presents the one dimensional modeling of of the process has to be capable of real-time operation

rotary kilns used for energy intensive production pro- anyway and thus, several assumptions and simplificacesses. Raw material is fed into an inclined rotating tions have to be done.

kiln and heated by counter current gas flow. Chemical

As a first step to the automatic control of continureactions take place in the bed of raw material as well ously operating rotary kilns, a detailed model of this

as in the gas phase. Heat and mass transfer between process is developed. The model abstracts from rethe bed and the gas phase are implemented. Also the ality by assuming one dimensional (1-D) counter curheat transfer to the environment is taken into account. rent flow of the raw material phase (bed phase) and the

As a benchmark, the process of limestone calcination gas phase. The bed and gas phase are surrounded by

is chosen. Results are compared with computational a combination of isolating refractory and steel shells.

fluid dynamic simulations.

Two reactions are implemented, one for the production

Keywords: CaCO3 , calcination, CFD comparison, of heat and one for the calcination itself. Methane is

kilns, limestone, rotary kilns, simulation

oxidized in the gas phase in order to supply the neces-

Introduction

products in chemical industry. The limestone calcination, as an energy intensive production process for

unhydrated lime, is often performed in continuously

operating rotary kilns. Until today, the process is manually operated and despite existing approaches the use

of automatic control is very uncommon. Due to the hot

and dusty atmosphere inside the drum, thermodynamic

states used as controlled variables by an expert system

are hardly measurable in a reliable way. In heat driven

chemical production processes such as limestone production measured data like a temperature as one thermodynamic variable of the process (often most easily

to measure) is not sufficient to estimate the chemical

rate of degradation of CaCO3 . To overcome this problem dynamic physical and chemical models can be applied to predict the behavior of dependent measures.

By comparing the results of the modeling to current

plant measurements the states of independent variables

in the bed phase consuming energy due to an endothermic degradation process. Heat and mass transfer take

place between the counter current flows and the environment. The paper is structured as follows: In chapter

2 the abstraction to 1-D counter current flow is shown.

Additionally, the mechanisms of reactions and heat

transfer are described. In chapter 3 the computational

results with Dymola are analyzed in detail. For validation, the results are compared to computational fluid

dynamics (CFD) simulations in chapter 4. Chapter 5

concludes the paper with an outlook of future investigation.

flows of gas and bed phase are counter current. The

rotary kiln itself consists of an isolation and a steel

shell. This abstraction is depicted in Figure 1.

814

DOI: 10.3384/ecp09430084

2.1

model of the Modelica fluid library [1]. It is extended

by dynamically changing cross sectional areas due to

bed heights. Replaceable models of radiative and convectional heat transfer are integrated and will be discussed in section 2.6. In addition, the gas phase is

equipped with a replaceable chemical reaction model

in order to cover the oxidation of mixed gaseous hydrocarbons (i.e. in this case Methane only), details are

covered in section 2.5.

The balancing equations with a dynamic momentum balance are formulated in [2]. Using a finite volume approximation and setting the momentum balance to be static, the equations (1)-(3), corresponding

to a single slice used in the DynamicPipe model, are

derived. To avoid obscurity, additional equations covering multi-component media are not given in this formulation.

dmi

dt

= m i+ 1 + m i 1 +

2

hydrocarbons are added to the RHS of the mass balance in equation (1). Including the heat of formation

of all components implicitly adds the contribution of

chemical reactions to the energy balance while only

considering mass balance changes. For the longitudinal gas flow and the heat transfer standard connectors

are used. For the gaseous exchange between gas and

bed signal oriented connectors for each direction are

designed using the same exchange medium (O2 , CO,

CO2 , H2 O).

All cross sectional areas, and hence corresponding

volumes, in these equations are dynamically changed

due to changes in bed height. Therefore, the information of the beds cross sectional area is transmitted via

input output relation to the gas phase. Finally, data

on gas phase properties are provided for other components by an output connector.

2.2

dmi

dt

m i+ 1 + m i 1 +

2

(4)

with m i+ 1 = iVi+ 1

2

dUi

(5)

= H i+ 1 + H i 1 +

2

2

dt

Heat and mass transfer is included similarly to gas

phase modelling via source terms to the RHS of the

balance equations. The transport of material through

the rotary kiln is specified by equation (6), which is

commonly known as Kramers equation [5].

(1)

)3

(

)(

2 2

4

tan

dh

h

h

i

i

3

2

2

2 i2

0 =

R R

Ai+ 1 pi+ 1 Ai 1 pi 1

2

2

(6)

) 2

( 2

The volume flow rate is a function of the rotation

+Ai pi+ 1 pi 1

2

2

frequency , the inner radius of the pipe R, the inclinaFFFV Ai i g z

tion of the kiln , the materials angle of repose , the

dUi

dh

= H i+ 1 + H i 1

(3) height of material h and the corresponding gradient dx .

2

2

dt

This differential equation in terms of the height is sim(

)

+vi Ai pi 1 pi+ 1 +

plified by rearranging and approximating the height

2

2

and the corresponding gradient with the equations (7)

for slice i = 1, . . . , n

to (9).

Source terms for heat, namely radiational and convectional contributions, are added to the right hand

hi = R (R cos (i /2))

(7)

side (RHS) of the energy balance in equation (3). Mass

dhi

di

= (R/2) sin (i /2)

(8)

transfer between bed and gas phase due to degradation

dx

dx

of CaCO3 (releases CO2 ) and changes in the compodi

(i+1 i ) / (L/n)

(9)

sition of the gas phase due to the oxidation of gaseous

dx

m 2i+ 1

m 2i 1

815

The error between the approximation and original

, the length of the rotary kiln by L and n is the number data pairs is given in Figure 2.

of slices in the rotary kiln. All geometric details for

gas and bed phase are calculated using the mid point

angle. The calculation of i = f (Ai ) is presented in

section 2.4.

2.3

The isolation and steel shells are modeled by an energy balance for the corresponding material volume

resulting from the 1-D balancing elements. Heat transfer, and hence the temperature profile, is realized using

Fouriers relation for heat conduction in solid material.

In principle, the shells are structured as grids consisting of heat capacitors and thermal conductors likewise

modeled in the modelica standard package. Heat transfer is possible in two directions, namely longitudinally

Figure 2: Approximation error for = f (P)

and transversely to the flow direction in the rotary kiln.

Geometric and material properties are parameters of

The adapted relationship = f (P) is implemented

the model. Standard heat connectors are used.

as a function and integrated in both the gas and bed

phase in order to calculate the mid point angle and

2.4 Mid point angle approximation

subsequently all geometric characteristics of the rotary

kiln.

All geometric properties for gas and bed phase can

easily be calculated using the mid point angle of the

bed phase. Nevertheless, the angle has to be calculated 2.5 Mechanism of chemical reactions

from the cross sectional area of the bed phase, which

is a direct result of the mass balance in every bed slice The replaceable chemical reaction model is designed

as a reactant limited elementary reaction using an Arof the rotary kiln. This is shown in equation (10).

rhenius type approach for the reaction kinetics. The

Ai = (mi /i ) / (L/n)

(10) reaction kinetics approach is shown with the equation

(14).

The relation between the cross sectional area Ai of

a single slice and the mid point angle i is implicitly

Ea

k = B T n e RT

(14)

given with the equations (11)-(12).

The preexponential coefficient B, the activation en(11) ergy Ea and n are free parameters which will be used

P = 2Ai /R2

(12) to fit the model to CFD simulation data. Generally

speaking, this fit is necessary since, on the one hand,

In order to avoid additional nonlinear equations, the no reliable chemical reaction data is available for such

relationship given with equation (11) is numerically a set up of coupled ideal reactors and, on the other

solved for in a range of P between 1.25 105 and hand, the model is not able to cope with local condi2. The corresponding pairs are then used for a least tions due to low resolution and the lack of adequate

square fit in order to find a good approximation for models. For example, the oxidation of mixed gaseous

= f (P). The function = f (P) is given with equa- hydrocarbons (i.e. in this case CH4 only) is mass transtion (13).

fer limited and therefore, an ideal mixed reactor needs

to be adapted using the averaged chemical reaction kinetics.

1

= a0 log(P) + a1 (1/P) + a2 P 2

The rate of degradation (massflow) for each com+a3 P + a4 P2 + a5 P3 + a6 P4

(13) ponent is calculated using the relationship given with

+a7 P5 + a8 P6 + a9

equation (15).

0 = P + (i sin i )

816

0.5 < Pr < 1.5, the simplified equation (21) can be

(15)

used.

k=1

m j = kV j M j Ckk

l

In this relationship, the velocity of reaction k is coupled with the volume of the reaction element V , the

molar mass M and the stoichiometric cofficient for

each component (index j over all components). The

approach is reactant limited assuming an elementary

reaction order. Hence, the molar density C to the

power of the stoichiometric coefficient sums up over

all reactants k of a reaction.

For the bed phase, the degradation of CaCO3 is implemented. The chemical reaction is given with equation (16).

CaCO3 = CaO +CO2

(16)

CH4 , equation (17) holds.

CH4 + 2O2 = CO2 + 2H2 O

(17)

as the defined medium covers all components and the

stoichiometric coefficients are defined.

2.6

For the heat transfer between the gas and bed phase

as well as the isolation shell convectional and radiational mechanisms are implemented. For convectional

heat transfer between the gas and its corresponding exchange partner, the heat transfer coefficient is dependent on the Reynolds number Re, the Prandtl number Pr and the Nusselt number Nu. The general convectional heat transfer equation in terms of is shown

with equation (18).

Q conv 12 = 12 A12 (T1 T2 )

[

( ) 23 ]

( 0.8

) 0.4

Dh

Nu = 0.0214 Re 100 Pr

1+

L

(21)

All the models calculate in a similar range from

8 10 W/m2 K.

Convectional heat transfer between the bed phase

and the isolation is also realized with the heat transfer coefficient and equation (18). is calculated

from various process parameters using two different

approaches which are described in detail in [8]. Typical values are said to be 50 200 W/m2 K

Also, models with constant are possible to

choose. The heat transfer models are designed to be

replaceable in order to enable the choice between different heat transfer mechanisms as described above.

Radiation between the bed, the gas and the isolation

is modeled using equation (22).

(

)

Q rad 12 = 12 A12 T14 T24

(22)

The referenced area for radiational heat transfer between transfer object 1 and 2 is given with A12 . The

emissivity coefficient 12 relates the visibilty between

area A12 and A21 and the emissivity of corresponding

objects. There are three emissivity coefficients to be

calculated, namely wall bed (wb), wall gas (wg)

and bed gas (bg). The formulas for calculating

these coefficients are given with equation (23) to (26).

(18)

interaction are implemented in the Modelica fluid

library [1]. Additionally, two relationships for Nusselt

numbers are given in [10]. The equations are shown

with (19) and (20).

w b (1 g )

U

w g (1 + (1 g ) (1 b ))

=

U

b g (1 + (1 g ) (1 w ))

=

U

= 1 (1 g ) (1 w )

wb =

(23)

wg

(24)

bg

U

(1 (1 (1 b ) (1 g )))

(25)

(26)

) 32 ]

free bed area (surface) and the free isolation area. De /8 (Re 1000) Pr

Dh

Nu =

(19) tails about the derivation can be found in [4]. The

(

) 1+

L

1 + 12.7 /8 Pr2/3

values of emissivity are almost constant over length x

= (1.82 log10 (Re) 1.64)2

(20) and temperature T with wb = 0.184, wg = 0.695 and

2300 < Re < 106 , Dh /L < 1

bg = 0.615.

[

817

Computational results

within the Dymola modeling environment. The set up

is depicted in the Figure 3.

increase of temperature and the endothermic character

of the calcination reaction. The increase of temperature for the main components of the rotary kiln (steel,

isolation, gas and bed phase) is depicted in Figure 5

The black and the grey objects denote the steel and

isolation shell, respectively, with different geometric

and material parameters. Inside the pipe, there is

counter current flow of the gas phase (blue element)

and the bed phase (limestone material, grey element).

Different mechansims for heat and mass transfer as

well as chemical reactions are chosen as described

earlier in this paper. Further components, e.g. crust

of semi liquefied limestone, can be added but are not

modeled in this contribution.

The calcination process (degradation of CaCO3 ) is

shown in Figure 4.

The system is initialized at 273.15 K and atmospheric pressure (time [s]: 0-3000). In a next step, the

system is brought to the operating point by increasing

temperature of the incoming mass flows of the bed and

the gas phase (time [s]: 3000-13000). This procedure

is followed by the intial increase of the combustion

gas massflow (time [s]: 13000-250000, massflow step

[kg/s]: 0.1-1.2692). It is clear to see that the rate of

CaCO3 degradation intensifies as the temperature increases. A second step to the combustion gas massflow

is applied after 300000 seconds (massflow step [kg/s]:

1.2692-2.5392). Again, the degradation of CaCO3 increases. The increase of degradation, while applying

these steps to the combustion gas flow, is due to the

phase

While the gas phase (red) responds extremely fast

to the step in combustion gas massflow, the bed phase

(yellow) is slower. The isolation (turquoise) and steel

(blue) shell are even slower in their step response. The

different time constants of the process can be recognized by an exemplary inspection of Figure 6 to 7.

It is easy to observe the small time constant of the

gas response lying in the range of 10-200 seconds.

For the isolation shell, the time constant of reponse

lies in the range of 20000-30000 seconds. This explains the stiffness of the system and the necessity of

stiff numerical solvers for simulations. Furthermore,

these time constants correspond to the known time

constants from process industry, which implies that

818

Since this work mainly focuses on the 1-D model of

the limestone calcination process, only a short summary of the models used in the CFD simulations will

be given here.

4.1

model

freeboard in the kiln is bounded by the refractory and

the surface of the solid bed. The methane burner extends into the kiln on one end of the drum (Figure 8).

Figure 6: Temperature response of gas phase due to

combustion gas step

rotary kiln

Figure 7: Temperature response of isolation due to

combustion gas step

the dynamical behaviour of the model reliably represents the calcination process. Although the steady

state values of the operating point also correspond to

the known values from process industry, this modeling

approach is justified even more by comparing its values to CFD simulation results in the following chapter.

Computational fluid dynamics (CFD) is a widely accepted tool for the detailed description of gaseous

combustion phenomena occurring within a rotary kiln

[6],[3]. Unfortunately, it does neither allow for the

modeling of transport of the solid bed nor for the theoretical description of the chemical reactions therein. In

the current work, different sub-models have been integrated in the commercial CFD code Fluent in order to

model the dynamics of the granular flow of the lime-

Steady state conservation equations of the compressible gas flow are solved considering the realizable k--model for turbulent effects in the gas phase.

Transport of four separate species (O2 , CH4 , CO2 and

H2 O) is calculated explicitly in the gas phase, while

the fifth one (N2 ) sums to unity. Combustion rates

of methane oxidization are assumed to be limited by

the mixing of turbulent eddies and thus, the eddydissipation model is used to predict reaction rates of

the volumetric reactions in the gas phase. Energy

transport phenomena include conduction, convection

and radiation (P-1 model), while the latter plays the

major role in rotary kiln processes. Absorption of the

gas mixture is mainly affected by the product constituents of the gas (CO2 and H2 O). Therefore the

wsggm-cell-based model is applied to calculate the local absorption coefficient of the gas mixture. A significant amount of energy discharges into the environment. Conduction driven heat transfer through the refractory is being calculated explicitly by applying a

computational grid to this region also. On the outer

819

considered: convection and radiation.

Thermal coupling between gas and solid phase is realized by setting a temperature profile on the bed surface. For this purpose mass, species and energy conservation equations within the particulate solid bed are

solved by implementing a mathematical submodel for

the solid bed. Since it has recently been proven, that

axial mixing can be neglected in industrial rotary kiln

processes, transport of the solid bed can be simplified

by assuming a plug flow [9]. Additionally the bed is

assumed to be well mixed locally in any given cross

section.

Limestone calcination can be modeled as a shrinking core process with surface reaction control according to equation (27) [7].

(

)

dmCaCO3

EA

= k0 exp

4 r2p Np MCaCO3

dt

R Tp

(27)

Herein r p and Np represent the mean particle radius and the total number of limestone particles, respectively. CO2 released by the calcination reaction is

assumed to be transported instantaneously to the hot

flow by neglecting any transport resistance in the solid

bed. It is released in the computational space of the

hot gas flow by adding mass and species sources in the

cells adjacent to the bed surface.

In Figure 9 the contour plot of the local gas temperature on the center plane is shown as an exemplary

result of the CFD simulations.

the center plane in [K]

In order to justify the 1-D abstraction of the process

modeled within the Dymola environment, the computational results are compared to the highly resolute results of the CFD simulations. For this purpose, volume

V, j of the CFD simulation data

based average values

are calculated for a discrete number of slices in the gas

phase. Due to the strongly anisotropic flow field in the

vicinity of the burner mass and velocity weighted average has to be applied for the potential variables. This

is shown in equation (28).

Av

V, j = Ncells i i i i,ax

Ncells i Ai vi,ax

(28)

cell inside the discrete slice and vi,ax as the local axial

velocity of the gas mixture are used to calculate the

volume based average of slice j for each scalar .

Since plug flow has been assumed in the clinker bed,

equation (28) can be simplified to the volume weighted

average for all potential variables in the solid phase as

given in equation (29).

Ncells i Vi

s

V,

j=

Ncells Vi

(29)

need to be integrated within each single control volume in the gas and in the solid domain, respectively.

For these data equation (30) is valid.

V, j =

(30)

Ncells

4.2

Comparison

chosen to be equal in both simulation environments.

In addition, the free chemical reaction parameters

(B, n, Ea ) for adapting the model are fitted to CFD simulation data by applying a least square fit using equation (15). Therefore, the CFD simulation data are concentrated in larger 1-D cells by applying the above described weighting functions. After model adaption via

least square fit, a Dymola simulation to steady state is

performed. The simulated data from the Dymola simulation environment are then compared to the weighted,

concentrated CFD simulation data. The essential values of the process are compared. This includes temperature profile of gas and bed phase, molar densities

of O2 and CH4 in the gas phase as well as molar density of CaCO3 in the bed phase (controlled variable for

future model predictive control).

Figure 10 shows the temperature profiles of the gas

phase for Dymola and CFD simulation.

In the next figure (Figure 11), the consumption of

O2 and CH4 is depicted.

The figures show a similar behaviour of the gas

phase in both simulation environments. For the error

e holds e < 2%. On first inspection, this seems to be

a good result. Nevertheless, the more relevant data for

intended controlling of the rotary kiln process is the

temperature and the concentration of components in

820

Figure 11: Comparison of gas phase molar density of Figure 13: Comparison of bed phase molar density of

O2 and CH4

CaCO3

the bed phase. Figure 12 shows the temperature of the

bed phase.

Despite the different scaling of the graph, for the error e holds e < 3%. The next figure (Figure 13) shows

the degradation of CaCO3 in the bed phase using the

molar density as depicted variable. The maximum error for the molar density of CaCO3 is e = 6.6%. Although this value is slightly higher than the previous

errors, the 1-D modeling approach is successfully applied. Various alternative values of the process were

compared, yielding to the same outcome. The main

advantage of the 1-D modeling approach is the possiblity of faster simulations while deviations are kept

small enough in the scope of robustness in terms of observer based model predictive control. While the simulation until convergence in the CFD environment takes

up to several days, the simulation of the Dymola model

takes seconds to minutes depending on the change of

input variables. Another enormous advantage of the 1-

physical abstraction. Since the identified data based

models are only valid in the range of measured data,

the nonlinear 1-D model of the rotary kiln will have a

wider range of validation. Furthermore, the simulated

data sets are always open to physical interpretation and

hence, are easier to check for plausibility.

Outlook

In a first step, the complex counter current flow process of rotary kilns is modeled and applied to the limestone degradation. First results show reasonable behaviour of the process physics. The comparison to

CFD simulation data confirms these results. The essential process parameters are compared and the errors

are small enough to allow for application in observer

based model predictive control application. In addi-

821

tion, the modeling approach has a lower computational [8] A. Queck. Untersuchung des gas- und wandseitigen Wrmetransportes in die Schttung von

burden and results in linearizations which are capable

Drehrohrfen. PhD thesis, Otto-von-Guerickeof real-time application in an expert system.

Universitt Magdeburg, 2002.

For the future, details in both models will be refined

in order to get even better results. Furthermore, the

model is going to be enhanced with a particle burner [9] R.G. Sheritt, J. Chaouki, A. Mehrotra, and L. Behie. Axial dispersion in the three-dimensional

and applied to the chemically more complex cement

mixing of particles in a rotating drum reactor.

production process. The task of automatic least square

Chemical Engineering Science, 58(2):401415,

fit for the free chemical parameters of the model will

2003.

be enhanced in order to cover the more complex cement production process. A detailed report on both [10] VDI-Gesellschaft

Verfahrenstechnik

und

topics will soon be published. Alongside with the enChemieingeniuerwesen,

editor.

VDIhanced model, linearizations of the nonlinear model in

Wrmeatlas. Springer, 8th edition, 1997.

desired operating points will be derived. Using these

linearizations, an observer for immeasurable process

values will be established. Furthermore, a model pre- 6 Acknowledgement

dictive control will be designed in order to hold a deThe authors gratefully thank the Federal Ministry

sired operating point of the plant.

of Education and Research for funding BMBF 3257

MoProOpt.

Furthermore, we highly appreciate

References

the supervision by the Project Management Agency

Forschungszentrum Karlsruhe (PTKA).

[1] F. Casella, H. Tummescheit, and M. Otter.

Modelica fluid library

www.modelica.org/libraries/

modelica_fluid/releases/1.0, 2009.

[2] H. Elmqvist, H. Tummescheit, and M. Otter.

Object-oriented modeling of thermo-fluid systems. Modelica Association, November 2003.

[3] M. Georgallis, P. Nowak, M. Salcudean, and

I.S. Gartshore. Modelling the rotary lime kiln.

Canadian Journal of Chemical Engineering,

83(2):212223, 2005.

[4] R. Jeschar, R. Alt, and E. Specht. Grundlagen

der Wrmebertragung. Viola-Jescher Verlag,

1990.

[5] H. Kramers and P. Croockewit. The passage

of granular solids through inclined rotary kilns.

Chemical Engineering Science, 1(6):259265,

1952.

[6] F. Marias, H. Roustan, and A. Pichat. Modelling

of a rotary kiln for the pyrolysis of aluminium

waste. Chemical Engineering Science, 60:4609

4622, 2005.

[7] K.S. Mujumdar, K.V. Ganesh, S.B. Kulkarni,

and V.V. Ranade. Rotary cement kiln simulator

(rocks): Integrated modeling of pre-heater, calciner, kiln and clinker cooler. Chemical Engineering Science, 62:25902607, 2007.

822

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